Abundant novel physical properties have been observed in thin-flake samples of two-dimensional correlated electronic systems prepared by mechanical exfoliation. Developing new methods of preparing bulk two-dimensional samples can further understand the low-dimensional system by combining traditional bulk characterization methods like X-ray diffraction, magnetic susceptibility and specific heat measurements. It is possible to maintain the novel properties of thin-flake samples in bulk state and promote these novel physical properties for potential applications. This article introduces a class of organic molecular intercalation methods to regulate two-dimensional correlated electronic systems, focusing on the changes of structure and physical properties of two-dimensional materials after organic molecular intercalation. The applications of organic molecular intercalation method in regulating thermoelectricity, two-dimensional magnetism, charge density wave and two-dimensional superconductivity are also presented.